APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Yuelong Xu,Ran Wang,Yuxuan Zheng,Lihui Zhang,Tifeng Jiao,Qiuming Peng,Zhenfa Liu
Because of their high catalytic activity and abundant resources, nonprecious transition metal phosphides are favorable substitutes for noble metals as hydrogen evolution reaction (HER) electrocatalysts. In this work, self-assembled Ni/Co phosphide composite N-doped carbon spheres were successfully prepared via a hydrothermal process, which had abundant exposed active sites for the HER. The as-obtained samples exhibited excellent electrocatalytic activity for the HER with an overpotential of only 160 mV (vs. RHE) at a current density of 10 mA cm −2 in a 0.5 M H 2 SO 4 solution and a comparatively low Tafel slope (57 mV dec −1 ). Additionally, the Ni 2 P/CoP spheres also show good stability after 120 h and 5000 cycles of a cyclic voltammetry test. Their highly efficient catalytic activity for the HER is attributed to the specific spherical structure, which provides exposed Ni 2 P and CoP for favorable adsorption and desorption of hydrogen. Therefore, nonprecious transition metal phosphide spheres may provide a promising strategy to improve the catalytic activity of HER electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2017
·
IF 12.343
Aiping Wu,Ying Xie,Hui Ma,Chungui Tian,Ying Gu,Haijing Yan,Xiaomeng Zhang,Guoyu Yang,Honggang Fu
Developing the efficient and low-cost electrocatalysts for overall water splitting is of the great importance for the production of H 2 . The popular bi-functional catalysts usually shown good activity for one half reaction at expense of the activity for another half-reaction, thus given a moderate performance for overall water splitting. In this paper, we have reported on integrating the active OER (Ni 3 N) and HER (NiMoN) components as Ni 3 N-NiMoN heterostructures for the effective overall water splitting. The heterostructures were constructed by the controllable nitridation of the Ni-Mo-O precursor anchored on carbon cloth (CC) under NH 3 atmosphere. The micro-structures of the catalyst could be tuned by regulating the surface properties of CC and the calcination temperature. Under optimized condition, the Ni 3 N-NiMoN catalysts exhibited good catalytic activity for both OER and HER in alkaline electrolyte . The catalysts can achieve a current density of 10 mA cm −2 at an overpotential of 31 mV for HER, being close to Pt catalyst. Also, it only requiring an overpotential of 277 mV to reach current density of 10 mA cm −2 for OER. Moreover, the cell assembled by the identical Ni 3 N-NiMoN as both the cathode and anode needs only a cell voltage of 1.54 V to achieve current density of 10 mA cm −2 . The superior performance of Ni 3 N-NiMoN heterostructures can be ascribed to the following points: 1) the simultaneous presence of active OER and HER components and the promoted action each other in the heterostructures, and 2) the exposure of the abundant active sites in the sheet-like structure assembled by the nanoparticles .
研究领域:
材料科学
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电化学
·
催化
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 24
·2201896
·
IF 15.153
Daying Guo,Zhixin Wan,Guoyong Fang,Mengqi Zhu,Bin Xi
Reported herein is a highly active and durable hydrogen evolution reaction (HER) electrocatalyst, which is constructed following a tandem interface strategy and functional in alkaline and even neutral medium (pH ≈ 7). The ternary composite material, consisting of conductive nickel foam (NF) substrate, Ni 3 S 2 -MoS 2 heterostructure, and TiO 2 coating, is synthesized by the hydrothermal method and atomic layer deposition (ALD) technique. Representative results include: (1) versatile characterizations confirm the proposed composite structure and strong electronic interactions among comprised sulfide and oxide species; (2) the material outperforms commercial Pt/C by recording an overpotential of 115 mV and a Tafel slope of 67 mV dec −1 under neutral conditions. A long-term stability in alkaline electrolytes up to 200 h and impressive overall water splitting behavior (1.56 V @ 10 mA cm −2 ) are documented; (3) implementation of ALD oxide tandem layer is crucial to realize the design concept with superior HER performance by modulating a variety of heterointerface and intermediates electronic structure.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Dongkui Huo,Zhichao Sun,Yingya Liu,Zhiquan Yu,Yao Wang,Anjie Wang
Tungsten phosphide (WP) is believed to be a promising electrocatalyst in the electrochemical hydrogen evolution reaction (HER) for its unique catalytic performances. Nevertheless, its further application is severely limited by the agglomeration caused by the high preparation temperature (over 600 °C). Herein, we adopt a citric acid-guided two-stage aging method to prepare Co-doped WP with small particle size and higher dispersity on the surface of seven different carbon supports. Co is successfully incorporated into the lattice of WP, causing preferable catalytic performance. The introduction of seven different carbon supports enhances electronic metal-supported interaction and proves this two-stage aging method universal. The as-derived CoWP-CA/KB (two-step aging) featured a low overpotential of 111 mV to achieve a current density of 10 mA cm–2, along with a desirable Tafel slope of 58 mV dec–1, outperforming most of the WP-based electrocatalysts. Besides, the electrode possesses excellent stability for 60 h without significant attenuation. Its remarkable performance results from its structure (delicate particle size, uniform dispersion, and large specific surface area) and its electrocatalytic properties (large electrochemically active surface area, excellent electrical conductivity, enhanced interfacial charge transfer kinetics, and high turnover frequency). This novel synthesis strategy will be pivotal for designing robust non-noble metal-based electrocatalysts with high HER activity and durability to meet the future keen demand for hydrogen.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 47
·21677-21684
·
IF 3.3
Xiaohao Jiang,Rongtao Xiao,Honggui Wang,Ya Zhang
As a high calorific and zero carbon energy source, hydrogen has received a significant amount of attention in recent years. In this work, the amorphous molybdenum sulfide was uniformly and orderly wrapped around the surface of Ni9S8/NF nanowires by electrodeposition to obtain a-MoSX@Ni9S8/NF nanoflower rods. A low overpotential of 138 mV (@10 mV cm−2) at room temperature was achieved for a-MoSX@Ni9S8/NF with a high electrochemically active surface area. An external thermal field could reduce the interfacial charge transfer resistance between the electrode and the electrolyte and promote the electrochemical hydrogen evolution reaction (HER). The a-MoSX@Ni9S8/NF showed excellent hydrogen precipitation performance of 72 mV (@10 mV cm−2) under 80 °C. The a-MoSX@Ni9S8/NF owned good reproducibility and durability after 5000 cycles in acidic media. The Faraday efficiency of the composite can reach 92.6%. This work provided a meaningful perspective on the design of electrochemical HER catalysts and external field assisted HER.
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DOI
高影响因子
Nanoscale
·
2020
·Vol. 12
·期 16
·9246-9254
·
IF 6.895
Junxiao Huang,Xuelei Pan,Xiaobin Liao,Mengyu Yan,Bruce Dunn,Wen Luo,Liqiang Mai
1T-MoS2 is widely used in the hydrogen evolution reaction (HER) due to its abundant active sites and good conductivity. However, 1T-MoS2 is thermodynamically metastable due to the distorted crystal structure. Recently, researchers have detected the J1 and A1g Raman peaks after the HER process and confirmed that the 2H–1T phase possesses good stability. Therefore, continuous HER is likely to transform 1T-MoS2 into a stable 2H–1T mixed phase. The in situ characterization of 1T-MoS2 individual nanosheets in the HER process is important to understand the intrinsic electrocatalytic behaviour at confined nanoscale, which has rarely been investigated. Herein, we built an individual 1T-MoS2 nanosheet micro–nano device by the intercalation of N-butyllithium into 2H-MoS2. Then, the device was kept at an overpotential (η) of 450 mV, which was much lower than the onset potential, for 20 minutes to ensure continuous HER. Through this electrochemical treatment, we successfully obtained a mixed phase of 2H–1T and monitored the electrochemical phase transition by in situ Raman mapping and atomic force microscopy (AFM). The HER performance of the 2H–1T phase was superior to that of 1T-MoS2 and 2H-MoS2. Additionally, computational simulations demonstrated that the 2H–1T phase exhibited optimal hydrogen adsorption energy. The presented work displays the excellent catalysis of the mixed phase obtained by the electrochemical phase transition, which provides new directions for improving the catalytic activity of TMDs.
研究领域:
材料科学
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电化学
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纳米技术
✓ 已验证
DOI
高影响因子
ACTA MATERIALIA
·
2025
·
IF 9.3
Xianqiang Yu,Ruikai Qi,Linfeng Zhang,Li Deng,Mengxiao Zhong,Zheng-jie Chen,Xiaofeng Lu
Constructing high-performance bifunctional electrocatalysts for water electrolysis under an ampere-grade current density is crucial for practical application. Herein, ruthenium-cobalt oxide (RuCoO x ) solid solution nanofibers (SSNFs) are fabricated as robust bifunctional electrocatalyst for both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). Typically, the optimized Ru 2 Co 1 O x SSNFs exhibit an ultra-low overpotential of 362 mV at 1000 mA cm -2 for OER, not only significantly superior to the prepared RuO x nanofibers (NFs), CoO x and commercial RuO 2 catalyst but also outperforming many reported typical OER electrocatalysts. In addition, the representative Ru 1 Co 1 O x SSNFs catalyst presents a good HER performance with an overpotential of only 149 mV at 1000 mA cm -2 and excellent stability over 120 h, surpassing the benchmark Pt/C catalyst. Furthermore, these catalysts are assembled to construct an alkaline overall water splitting cell, demonstrating a better performance than most of the recently reported water electrolyzers. Density functional theory calculations reveal that the addition of Co effectively modulates the d -orbitals of Ru and reduces the reaction energy barriers of O*→OOH*, benefitting to enhance the OER property. Additionally, the hybridization of Co and Ru is beneficial for modulating the strength of H* adsorption in an alkaline solution, which promotes the alkaline HER efficiency.
研究领域:
材料科学
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催化化学
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能源转换
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Ruoyu Wei,Mansheng Liao,Lidan Sun,Qingfeng Zhang,Hong Zhang,Lei Zhang,Zhongxin Song
Developing highly efficient and low-cost bifunctional electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in water splitting poses significant challenges. In this study, a novel bifunctional electrocatalyst, Irn-CoMoPOx, was achieved via incorporating low-loading Ir single atoms and clusters with the high-valence Mo6+ modified CoPOx nanosheets. The Irn-CoMoPOx catalyst demonstrates remarkable low overpotentials of 222 mV and 36 mV for the OER and HER, respectively, in delivering a current density of 10 mA cm–2. When employed as both the anode and cathode catalyst in overall water splitting, the Irn-CoMoPOx∥Irn-CoMoPOx configuration exhibits a superior cell voltage of 1.53 V, outperforming the benchmark Pt/C∥IrO2 electrolytic cell (1.60 V) for achieving the current density of 10 mA cm–2. Benefiting from the high-valence of Mo species, the metal–support interaction of Irn-CoMoPOx was greatly strengthened, resulting in an order of magnitude increase in the mass activity of Ir for the HER. The high valence of non-noble metals plays a crucial role in tuning the local electronic configurations and optimizing the adsorption energies of the intermediates, which synergistically improves the overall performance of Ir in water splitting. The study provides valuable insights for future research in the utilization of Ir-based bifunctional catalysts for overall water electrocatalysis applications.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Shipeng Geng,Liming Chen,Yinlong Wu,Yi Wang,Shuqin Song
Designing efficient and durable hydrogen evolution reaction (HER) catalysts for seawater electrolysis is crucial for large-scale hydrogen production. Here, we introduce a theory-driven design of metal/WN electrocatalysts, with metal strongly coupled to lattice-matched WN. Theoretical calculations for Pt/WN reveal that W sites enhance H 2 O adsorption/dissociation, optimizing Pt’s H binding. The prepared Pt/WN@CP nanorod can catalyze HER with low overpotentials of 107 and 113 mV at 500 mA cm −2 in alkaline water/seawater, respectively, surpassing Pt/C. Extended calculations and experiments show that the optimized Ni/WN@CP-90 achieves an optimal Δ G H* and overpotential of 219 mV at 500 mA cm −2 in alkaline seawater, demonstrating the versatility of the WN support to promote HER activity. Notably, the anion exchange membrane water electrolyzer (AEMWE) constructed by Pt/WN@CP or Ni/WN@CP-90 with NiFe-LDH@NF demonstrates outstanding hydrogen production activity with excellent Faraday efficiency (∼100%) and durability (120 h), indicating the potential application of WN-supported catalysts for efficient, stable seawater electrolysis.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Energy
·
2020
·
IF 5.604
L. Zheng,W. Zhang,B. Gao,H. Lu,X. Fan,Y. Zhang,Y. Wang,S. Wang,Q. Gao,Y. Tang
Transition metal dichalcogenides (TMDs) are regarded as the inexpensive and stable electrocatalysts for hydrogen evolution reaction (HER). Designing an electrocatalyst with few-layered molybdenum disulfide (MoS 2 ) is one of the most effective methods to enhance the activity and durability for HER due to its abundant exposed rim-sites, fast electron transfer and high chemical stability. Herein, a green and facile one-pot approach is developed to synthesize few-layered MoS 2 /nitrogen, sulfur codoped porous carbon (MoS 2 /NSPC) electrocatalyst via pyrolyzing the in-situ formed molybdate-melamine complex (MoO x -MEL) within the self-assembled networks of melamine-trithiocyanuric acid (MT). The optimal MoS 2 /NSPC electrocatalyst exhibits excellent HER stability and activity with overpotential of 114 mV at 10 mA cm −2 in 0.5 M H 2 SO 4 . Furthermore, few-layered tungsten disulfide anchored on N, S-codoped porous carbon (WS 2 /NSPC) with high HER activity can also be successfully synthesized by this strategy. It paves a universal way to design active sites–enriched few-layered dichalcogenides with high performance in the applications from energy conversion to storages.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Scientific Reports
·
2017
·Vol. 7
·期 1
·1-9
·
IF 4.259
Wang Tingting,Wu Liqian,Xu Xiaobing,Sun Yuan,Wang Yuanqi,Zhong Wei,Du Youwei
The development of efficient, universal and inexpensive electrocatalysts for hydrogen evolution reaction (HER) is central to the area of sustainable energy conversion. Considering the Co-based sulfides/phosphides have the same catalytic mechanism with the hydrogenases occurring in nature. Here, a new catalyst based on Co 3 S 4 /CoP hybrid that is comprised entirely cheap and earthabundant elements, was first synthesized via a two-step method, the Co(CO 3 ) 0.5 (OH)·0.11H 2 O precursor was prepared by a hydrothermal method, followed by phosphidation and sulphidation under Ar atmosphere simultaneously. The resulting Co 3 S 4 /CoP hybrid material possessed porous core-shell structure with a homogeneous element distribution and large electroactive surface area (~21.04 mF cm −2 ). More importantly, the nanostructured Co 3 S 4 /CoP electrode exhibits excellent HER properties in acid medium with a low onset overpotential of 34 mV, a small Tafel slope of 45 mV dec −1 , as well as a large exchange current density of 150 μA cm −2 . These results obtained in this study indicate that the Co 3 S 4 /CoP hybrid nanorod is promising replacement to the Pt-based catalysts for H 2 production. Moreover, the synthetic method presented in this work can provide an efficient way to synthesis other nanocomposites.
研究领域:
材料科学
·
能源转换技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Jianpo Chen,Qiuyan Jin,Yinwei Li,Yan Li,Hao Cui,Chengxin Wang
In alkaline media, the water-dissociation-related Volmer process always suppresses the hydrogen formation/desorption process, which makes it challenging to develop non-noble-metal alkaline electrocatalysts with excellent catalytic activity. Here, we proposed a two-pronged strategy to simultaneously promote the kinetic process of both water dissociation and hydrogen desorption with the Co-doped WO2/amorphous CoxW hybrid electrocatalyst. Impressively, the optimized hybrid exhibits an outstanding hydrogen evolution reaction (HER) activity with the quite small Tafel slope of 19.77 mV dec–1 and ultralow overpotential of just 25 mV to reach a current density of 10 mA cm–2 in alkaline media. Both experiments and density functional theory calculations reveal that the top-level HER performance can be attributed to the cooperation of two different active components, in which the water molecule can easily be activated on the amorphous CoxW with low energy barrier (ΔGw = 0.46 eV), while hydrogen atoms can rapidly desorb from the Co-doped WO2 with an optimal Gibbs free energy of hydrogen adsorption (ΔGH* = −0.06 eV). Also, the density functional theory calculation further confirms that the H* tends to combine with another H* via Tafel step rather than Heyrovsky step. The findings provide unique insights for the development of the state-of-the-art non-noble-metal HER electrocatalyst with a Pt-like kinetic behavior in alkaline media.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子